Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 26
·14793-14805
·
IF 12.732
Yuan Gao,Xiaoguang Duan,Bin Li,Qianqian Jia,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Shaobin Wang,Wenchao Peng
Persulfate-based advanced oxidation processes are promising technologies to solve water pollution. In this work, single iron atoms are anchored on three-dimensional N-doped carbon nanosheets by a chemical vapor deposition (CVD) method with ferrocene-loaded CaO as the hard template. The high surface density of Fe–N4 sites and abundant interconnected meso–macro pores are highly favorable for activating peroxymonosulfate (PMS) to produce superoxide radicals (O2˙−), giving rise to ultrahigh activity and excellent stability for pollutant degradation. Experiment and density functional theory (DFT) calculations reveal that Fe–N4 is the main active site, on which electrons transfer from C to Fe via the C–N–Fe bond to secure the low-valence state of Fe species for the redox process. This work proposes a new strategy for developing highly active single-atom materials by CVD and reveals mechanisms of PMS activation on single-atom activators.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yunqi Wang,Peng Zhou,Qingguo Wang,Xiaowei Huo,Xue Huang,Qian Ye,Hao Xu,Guanyu Zhou,Yuhang Liu,Jing Zhang
Hydroxylated fullerene, Fullerol, has applied in many areas because of its high electron affinity and antioxidant potential, while it was few used in wastewater treatment. In this study, the mechanism involved that Fullerol accelerated the regeneration of Fe(II) in the Fe(III)/H 2 O 2 system under dark condition, which was investigated with chloramphenicol (CAP) as a model pollutant. In Fullerol/Fe(III)/H 2 O 2 system, CAP removal was completely achieved at 60 min via a non-photochemical pathway. In addition, the quenching experiments and electron spin resonance (ESR) results indicated that hydroxyl radical ( OH) was the main reactive oxygen species (ROSs). The Fullerol/Fe(III)/H 2 O 2 system had a rate constant of CAP degradation about 5.0 × 10 −2 min −1 , which was about 22 times higher than it in Fe(III)/H 2 O 2 Fenton-like system (2.3 × 10 −3 min −1 ). Fe(II) was ascertained the effective component that was responsible for H 2 O 2 activation to produce OH, which derived from 1) the first pathway: Fullerol complexed with Fe(III) and the redox potential of the complex is much lower than Fe(III)/Fe(II); 2) the second pathway: Fullerol acted as an electron donor to reduce Fe(III) into Fe(II). Moreover, CAP degradation intermediates were identified and its degradation pathways were proposed. This study suggested a new approach for improving the Fe(III)/H 2 O 2 system by accelerating Fe(III)/Fe(II) cycles with Fullerol.
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Catalysts
·
2022
·Vol. 12
·期 11
·1435
·
IF 4.501
Fujian Yang,Cheng Yin,Mengqiao Zhang,Jiangwei Zhu,Xiuyuan Ai,Wenchao Shi,Guilong Peng
The activation of persulfate (PS) by Fe(III) for the removal of environmental organic pollutants was severely limited by the low reduction rate from Fe(III) to Fe(II). In present study, we reported that reducing sulfur species (i.e., SO32−, HSO3−, S2−, and HS−) under low concentration could significantly accelerate the Fe(III)/Fe(II) cycle in the Fe(III)/PS system. Under the condition of 1.0 mM Fe(III) and 4.0 mM PS, the removal performance of Fe(III)/PS system was poor, and only 21.6% of BPA was removed within 40 min. However, the degradation efficiency of BPA increased to 66.0%, 65.5%, 72.9% and 82.7% with the addition of 1.0 mM SO32−, HSO3−, S2−, and HS−, respectively. The degradation efficiency of BPA was highly dependent on solution pH and the concentration of reducing sulfur species. When the reductant was excessive, the removal efficiency would be significantly inhibited due to the elimination of reactive species. This study provided some valuable insights for the treatment of organic wastewater containing these inorganic reducing ions.Keywords:persulfate;reducing sulfur species;cycle;degradation
研究领域:
环境科学
·
化学
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FOOD HYDROCOLLOIDS
·
2023
·
IF 10.7
Yuhuan Zhang,Beibei Wang,Chunmeng He,Lin Shi,Jianke Li
Iron deficiency is the utmost critical problem of nutrition worldwide. Polysaccharide-iron chelate is a promising iron supplementation that exhibits good stability, high absorption rate, and fewer adverse reactions, but it still owns drawbacks of extra energy and lower iron content with respect to inorganic ones. Carboxylated polysaccharide-iron has been proven with enhanced iron content, however with poor aqueous solubility. Here, Fe 3+ concentrations controlled highly soluble carboxylated inulin-iron chelates were synthesized to promote the sustained release and efficient supplement of iron with no extra energy. Inulin, soluble dietary fiber, was initially reacted with succinic anhydride (SA) to get carboxylated inulin (IN-SA) consequently enhancing the complexing ability of Fe 3+ and its bioavailability. Interestingly, the aqueous solubility of the IN-SA-iron chelate (IN-SA-Fe) directly correlated with the Fe 3+ concentrations. Relatively higher or lower Fe 3+ concentrations resulted in highly soluble IN-SA-Fe, otherwise, leading to insolubility precipitates. The possible mechanism was proposed as the polymerization reaction of IN-SA in different degrees with Fe 3+ acting as the cross-linker. Moreover, IN-SA-Fe was demonstrated with properties of sustained slow-release of iron in artificial gastric juice and good in vivo biosafety. This work provides a simple, efficient, no extra energy soluble iron supplement for the treatment of iron deficiency.
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CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Jie Liu,Chunmiao Liu,Yanchun Tong,Haibin Sun,Hui Peng,Mingwei Zhang,Shigang Wu,Hongying Zhang,Hongyu Gong,Zhiqin Zheng,Xue Guo,Yurun Feng
The SiCN/Fe/Ni ceramics codoped with iron acetylacetonate (FA) and nickle acetylacetonate (NA) was synthesized by polymer-derived ceramics (PDCs) method in this study. The microstructure, phase composition and electromagnetic wave (EMW) absorption properties of the samples were analyzed. The polarization loss and conduction loss of materials were analyzed by the direct current (DC) multimeter and the contribution rate of polarization loss was more than 94% in the whole frequency band. The results showed that C, SiC, Fe 2 Si, Ni 3 Si, γ- (Fe, Ni) and CNTs were formed after pyrolysis which provided lots of heterogeneous interface and enhanced the interfacial polarization. Meanwhile, Ni could enter the lattice of Fe and formed a unique electronic configuration, which reinforced the conductivity and stability of Fe. In addition, the in-situ generated Fe 2 Si and Ni 3 Si provided magnetic loss and conduction loss. The RL min value of SiCN/Fe/Ni-3 ceramic was −52.06 dB at 1.54 mm and the effective absorption band (EAB, RL ≤ −10 dB) reached 4.21 GHz (13.79–18 GHz, 1.43 mm).
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JOURNAL OF CATALYSIS
·
2026
·
IF 6
Zhengxi Zou,Zhenke Xu,Weiming Hua,Yinghong Yue,Zi Gao
Catalytic ethane dehydrogenation to ethylene is an attractive route for ethylene production following the shale gas revolution. However, its industrial implementation remains challenging due to high costs and environmental concerns. Iron-based catalysts have been identified as promising alternatives, while their catalytic performance is significantly dependent on the coordination environment and oxidation state of the iron species. Herein, a series of Fe/ZSM-5 catalysts were synthesized via urea precipitation (FeZ-P) and incipient wetness impregnation (FeZ-I) methods to investigate the relationship between Fe species evolution and catalytic behavior during ethane dehydrogenation. The FeZ-P catalysts exhibited significantly enhanced activity compared with FeZ-I, which was attributed to the improved dispersion of iron species and their favorable transformation behavior under reaction conditions. Detailed characterizations of fresh and spent catalysts revealed that the initial Fe 2 O 3 species on FeZ-P surface possessed limited dehydrogenation activity but underwent reaction-induced reduction and carbonization, generating Fe 3 C with enhanced ethane dehydrogenation performance. In contrast, the Fe 2 O 3 bulks on FeZ-I exhibited slower transformation rates, resulting in inferior catalytic activity. Air oxidation treatment enabled partial regeneration of the catalyst by removing carbon deposits and modifying Fe species evolution. This study highlights the importance of regulating Fe species dispersion and dynamic reduction-carbonization behavior, through which catalytically active Fe 3 C can be generated for enhanced ethane dehydrogenation performance. These findings provide valuable insights into the rational design of efficient Fe-based catalysts for non-oxidative alkane dehydrogenation.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2023
·
IF 5.2
Ning Gu,Yueyang Xu,Yan Yin,Xuzhao Gao,Yongping Zeng
SO x released from the combustion of sulfur-containing compounds in fuels pollute the environment and have a serious impact on human health. Adsorption desulfurization is an effective and environmentally friendly technique for removing sulfur-containing compounds from fuels. Metal-organic frameworks (MOFs) have high specific surface areas and can be easily modified and functionalized, making them excellent candidates for adsorption desulfurization in fuels. In this work, the precursor MIL-100(Fe)-SA was prepared using the hydrothermal method , and the adsorbent Ni@MIL-100(Fe)-SA was obtained by doping Ni 2+ into the resulting MIL-100(Fe)-SA using the impregnation method. FT-IR, X-ray diffraction, scanning electron microscopy, transmission electron microscopy and nitrogen adsorption-desorption isotherms were used to analyze the samples. The results indicated that Ni 2+ was successfully loaded onto MIL-100(Fe)-SA, and the MOF's structure remained stable. The adsorption performance of benzothiophene and thiophene was evaluated through batch adsorption experiments. The adsorption capacities of Ni@MIL-100(Fe)-SA for thiophene and benzothiophene were 23.68 mg S/g and 49.58 mg S/g, respectively. These observations could be ascribed to the π-complexation interactions between Ni 2+ of the framework and thiophenic compounds. The regeneration experiments demonstrated that the spent 11Ni@MIL-100(Fe)-SA-1.5 reach 86% of the adsorption capacity of fresh adsorbent after four cycles. Additionally, the regenerated adsorbent maintained good crystallinity after recycling.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Jin Huang,Jie Cao,Ni Tu,Huaping Dong,Jianfa Li,Jianxin Shou,Yimin Li
Nonionic and anionic surfactants often occur in anaerobic environments, but their roles in the removal of organic contaminants by Fe-bearing mineral/Fe(II) have not been determined. In this study, batch experiments were performed to investigate the effects of a nonionic surfactant (TX-100) and an anionic surfactant (SDBS) on the removal of nitrobenzene (NB) by Fe-bearing montmorillonite (FM)/Fe(II). Mössbauer spectrum and XPS were applied to analyze the edge surface bound Fe(II) and secondary minerals formed on FM. The contribution of surfactant to the enrichment of NB on FM was studied. The results showed that TX-100 and SDBS had opposite effects on the removal of NB by FM/Fe(II) at neutral pH. The presence of TX-100 improved the removal efficiency of NB from 36.4% to 70.0%, and increased the initial removal rate by 1.7 times. This enhancement effect was mainly attributed to the formation of more active edge surface bound Fe(II) that can reduce more NB to aniline. Formation of more magnetite on FM and selective enrichment of NB on the reactive surface also contributed to the removal of NB. In contrast, the presence of SDBS reduced the amount of edge surface bound Fe(II) via formation of SDBS-Fe(II) complex, which decreased the removal efficiency of NB.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jialong Yin,Heng Zhang,Mengfan Luo,Jia Zhao,Bingkun Huang,Pinji Chen,Zhenpeng Cai,Yue Yuan,Yang Liu,Chuanshu He,Bo Lai
The ferrous species (Fe(II))-periodate (PI) system employs efficient decontamination by generating ferryl species (Fe(IV)-oxo) under acidic pH conditions. However, the mechanisms by which the Fe(II)/PI system operates across a broad pH range remain elusive. In light of the rapid oxidation and consumption of Fe(II) at neutral pH, we developed an electro-Fe(II) system utilizing an iron plate anode to activate PI (E(Fe/C)/PI). Efficient sulfamethoxazole (SMX) degradation was achieved under the E(Fe/C)/PI system across a range of pH values. Quenching and chemical probe experiments revealed a transition from Fe(IV)-oxo to singlet oxygen ( 1 O 2 ) as the predominant reactive species from acidic to near-neutral pH, respectively. Density functional theory (DFT) calculations indicated that the differences in one-electron transfer capacity and hydrolysis pathways for various protonated Fe(IV)-oxo species underlie the variations in catalytic mechanisms. This study not only enhances the efficiency of the Fe(II)/PI system but also provides a comprehensive understanding of the activation mechanisms at different pH levels.
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iScience
·
2022
·
IF 6.107
Zheng Qian,Lingzhen Wang,Mawuli Dzakpasu,Yujia Tian,Dahu Ding,Rongzhi Chen,Gen Wang,Shengjiong Yang
The mechanism of spontaneous Fe III /Fe II redox cycling in iron-centered single-atom catalysts (I-SACs) is often overlooked. Consequently, pathways for continuous SO 4 ·- /HO⋅ generation during peroxymonosulfate (PMS) activation by I-SACs remain unclear. Herein, the evolution of the iron center and ligand in I-SACs was comprehensively investigated. I-SACs could be considered as a coordination complex created by iron and a heteroatom N-doped carbonaceous ligand. The ligand-field theory could well explain the electronic behavior of the complex, whereby electrons delocalized by the conjugation effect of the ligand were confirmed to be responsible for the Fe III /Fe II redox cycle. The possible pyridinic ligand in I-SACs was demonstrably weaker than the pyrrolic ligand in Fe III reduction due to its shielding effect on delocalized π orbitals by local lone-pair electrons. The results of this study significantly advance our understanding of the mechanism of spontaneous Fe III /Fe II redox cycling and radical generation pathways in the I-SACs/PMS process.
研究领域:
催化
·
环境化学
·
材料科学
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2026
·
IF 9.2
Lu Zeng,Xuexia Guo,Jiahao Sun,Wenbin Huang,Huinan Zhao,Lingling Hu,Shuanghong Tian,Chun He
In Fenton-like processes, achieving rapid and efficient redox cycling of metal active centers remains a challenge. This study presents an innovative strategy that harnesses the mechanical energy of water flow to drive the redox cycling of metal active centers. Herein, Fe 3 O 4 /MoS 2 heterojunction with interfacial Mo-S-Fe bridge bonds was constructed via a one-step hydrothermal method. Under the stimulation induced by water-flow mechanical, the piezoelectric effect of MoS 2 generates charge carriers, which are rapidly directed to Fe active sites through the Mo-S-Fe bonds. This process significantly accelerates the Fe(III)/Fe(II) cycle and enhances H 2 O 2 activation, achieving 93.8% removal of sulfamethoxazole (SMX) within 60 min under water flow stimulation. The composite exhibits robust performance across a broad pH range (3.0-10.7) and in the presence of humic acid (HA) and coexisting anions, demonstrating its strong environmental adaptability. Spectroscopic evidence confirmed the formation of Mo-S-Fe bonds at the heterojunction interface. Mechanistic studies further revealed that the structure improves charge separation, promotes rapid electron transfer from MoS 2 to Fe sites, and strengthens H 2 O 2 adsorption, thereby synergistically boosting reactive oxygen species (ROSs) generation and the overall catalytic efficiency. This study proposes an innovative strategy that exploits mechanical forces generated by water flow to drive rapid redox cycling of active metal centers in Fenton-like reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Feng Cheng,Peng Zhou,Xiaowei Huo,Yang Liu,Yunxin Liu,Yongli Zhang
The photocatalytic behavior of the graphene oxide (GO) modified Fe(III)/peroxymonosulfate (Fe/PMS) system for bisphenol A (BPA) degradation was investigated. With the addition of GO, a dramatic enhancement of BPA degradation was obtained at pH 3.0 under visible light irradiation. According to ESR analysis and quenching tests, both SO 4 - and OH are responsible for BPA degradation. The characterization analysis demonstrates that Fe(III) can chelate with the oxygenic functional groups on the surface of GO forming a stable GO-Fe(III) complex. The detections of different kinds of Fe species reveal that Fe(III) can be reduced to Fe(II) by GO via intramolecular electron transfer in the GO-Fe(III) complex, and visible light could enhance this process. The Fe(III)/Fe(II) cycle not only occurs on the surface of GO, but also in aqueous solution via homogeneous reactions. In addition, the degradation pathway of BPA was proposed based on the identification of the intermediates using GC–MS and LC-MS techniques.
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